Cited by 63Electrocatalysts for Energy ConversionElectrochemical sensors and biosensorsCO2 Reduction Techniques and Catalysts

Mediating Self‐Oxidation and Competitive Adsorption for Achieving High‐Selective Urea Oxidation Catalysis at Industrial‐Level Current Densities

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Qiao, Pengfei, Li, Guorui, Xu, Xiujuan, Wang, Danni, Wang, Fangqing, Xu, Liangliang, Lu, Linguo, Cong, Hailin +1 more·2025·Advanced Functional Materials

Abstract

Inhibiting the deactivation of nickel‐based catalysts caused by self‐oxidation and competitive adsorption behavior is still a major challenge for urea oxidation reaction (UOR), especially under industrial‐level current densities. In this study, a crystalline NiSe 2 /amorphous NiFe‐LDH (NiSe 2 /NiFe‐LDH) heterojunction catalyst is rationally constructed for selective electrocatalytic UOR. In situ Raman spectra and ex situ characterization results reveal that such a structure can tailor the self‐oxidation of catalyst and impede the accumulation of NiOOH species during the UOR process. Density function theory simulations disclose that the self‐driven charge transport from electron‐deficient NiFe‐LDH region to electron‐rich NiSe 2 region would induce the formation of local electrophilic/nucleophilic region to adsorb the electron‐donating ‐NH 2 and electron‐withdrawing C = O groups, respectively. This optimizes the adsorption of urea molecules and hinders the overaccumulation of OH − ions on the surface of NiSe 2 /NiFe‐LDH, which is beneficial for the priority occurrence of UOR over the oxygen evolution reaction (OER) and the realization of high UOR selectivity. Benefiting from the tailored surface self‐oxidation and favorable urea adsorption, the NiSe 2 /NiFe‐LDH could act as a high‐selective UOR anode and achieve ultrahigh 800 mAcm −2 only at 1.447 V. Besides, UV–vis spectrophotometry also unveiled that the NiSe 2 /NiFe‐LDH has the capability to electrochemically degrade urea, offering great promise for practical application potentials.

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Authors
Qiao, P., Li, G., Xu, X., Wang, D., Wang, F., Xu, L., Lu, L., Cong, H., & Sun, M.
Affiliations
  • Ocean University of China (CN)
  • Shandong University of Technology (CN)
  • University of Puerto Rico at Río Piedras (PR)
Corresponding author
  • Xu, Xiujuan
  • Xu, Liangliang
  • Cong, Hailin
  • Sun, Mingliang
Venue
Advanced Functional Materials
Publisher
Wiley
Published
2024-12-23
Volume
35
Issue
17
ISSN
  • 1616-301X (ISSN-L)
  • 1616-3028
OpenAlex
W4405727487
Cited by
63
References
2
Citations by year
2026: 46 · 2025: 17
FWCI
4.20
Type
journal article
Language
en
Open access
Locations
Advanced Functional Materials (publishedVersion)
Funders
  • National Natural Science Foundation of China (52173291, 22074072, 22274083)
  • Natural Science Foundation of Shandong Province (ZR2024ME032, ZR2022LZY022, ZR2023LZY005)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Electrochemical sensors and biosensors
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
urea oxidation reaction, electrocatalysis, nickel selenide, NiFe layered double hydroxide, heterojunction catalysts, self-oxidation, competitive adsorption, urea adsorption, oxygen evolution suppression, urea degradation, high current density

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